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Low‐Threshold Amplified Spontaneous Emission and Lasing from Thick‐Shell CdSe/CdS Core/Shell Nanoplatelets Enabled by High‐Temperature Growth

DOI:10.1002/adom.201901615 期刊:Advanced Optical Materials 出版年份:2019 更新时间:2025-09-12 10:27:22
摘要: Colloidal semiconductor nanoplatelets (NPLs) have recently emerged as highly promising optical gain medium because of their superior optical properties. Here, the shell-thickness-dependent optical gain properties of CdSe/CdS core/shell NPLs synthesized by high-temperature growth are systematically investigated for the first time. The core/shell NPLs show the increased quantum yields and enhanced photostability as well as clear reduced emission blinking, thanks to the preferable passivation of nonradiative surface defects by the growth of the high-quality CdS shells under high reaction temperature. Meanwhile, the amplified spontaneous emission (ASE) performance of CdSe/CdS NPLs indicates a nonmonotonic dependence on the shell thickness. The ASE threshold is achieved as low as ≈4.4 μJ cm?2 for thick-shell NPLs with six monolayer CdS shells, and exhibiting ultrafast transient dynamics process (≈11 ps). Besides, an extremely long lifetime (>800 ps) and large bandwidth (>140 nm) of optical gain are observed by employing ultrafast transient absorption spectroscopy. Finally, a thick-shell NPLs vertical cavity surface-emitting laser is developed, which demonstrates spatially directional single-mode operation with an ultralow lasing threshold of ≈1.1 μJ cm?2. These excellent results are attributed to the remarkable optical gain performance of core/shell NPLs and represent an important step toward practical NPL laser devices.
作者: Lei Zhang,Hongyu Yang,Buyang Yu,Ying Tang,Chunfeng Zhang,Xiaoyong Wang,Min Xiao,Yiping Cui,Jiayu Zhang
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Investigating the shell-thickness-dependent optical gain properties of CdSe/CdS core/shell nanoplatelets synthesized by high-temperature growth for low-threshold amplified spontaneous emission and lasing applications.

The study demonstrates that thick-shell CdSe/CdS NPLs exhibit remarkable optical gain performance with ultralow ASE and lasing thresholds, long gain lifetimes, and large gain bandwidths, making them superior nanomaterials for optical gain and lasing applications. However, further optimizations are needed to improve gain performance and reduce lasing thresholds for continuous-wave pumped or electrically driven colloidal NPL lasers.

The study identifies that further optimizations are necessary to eliminate defects in ultrathick-shell NPLs, which may quench exciton transfer and weaken the suppression of Auger recombination, potentially hindering the building up of population inversion in the CdSe core.

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